Cardiorespiratory fitness is thought to have beneficial effects on systemic vascular health, in part, by decreasing arterial stiffness. However, in the absence of non-invasive methods, it remains unknown whether this effect extends to the cerebrovasculature. The present study uses a novel pulsed arterial spin labelling (pASL) technique to explore the relationship between cardiorespiratory fitness and arterial compliance of the middle cerebral arteries (MCAC). Other markers of cerebrovascular health, including resting cerebral blood flow (CBF) and cerebrovascular reactivity to CO₂(CVR_CO2) were also investigated. Eleven healthy males aged 21 ± 2 years with varying levels of cardiorespiratory fitness (maximal oxygen uptake ([Formula: see text]O_2MAX) 38–76 ml/min/kg) underwent MRI scanning at 3 Tesla. Higher [Formula: see text]O_2MAXwas associated with greater MCAC (R² = 0.64, p < 0.01) and lower resting grey matter CBF (R² = 0.75, p < 0.01). However, [Formula: see text]O_2MAXwas not predictive of global grey matter BOLD-based CVR (R² = 0.47, p = 0.17) or CBF-based CVR (R² = 0.19, p = 0.21). The current experiment builds upon the established benefits of exercise on arterial compliance in the systemic vasculature, by showing that increased cardiorespiratory fitness is associated with greater cerebral arterial compliance in early adulthood.